GSTDTAP  > 气候变化
DOI10.1126/science.abh3418
Role of the ionic environment in enhancing the activity of reacting molecules in zeolite pores
Niklas Pfriem; Peter H. Hintermeier; Sebastian Eckstein; Sungmin Kim; Qiang Liu; Hui Shi; Lara Milakovic; Yuanshuai Liu; Gary L. Haller; Eszter Baráth; Yue Liu; Johannes A. Lercher
2021-05-28
发表期刊Science
出版年2021
英文摘要Brønsted acidity is introduced into microporous zeolites through the addition of framework aluminum. Pfriem et al. show that in the presence of water, the limited volume in the microchannels of zeolite H-MFI leads to a high concentration of hydrated hydronium ions at aluminum sites. The resulting high charge density creates a highly non-ideal solvation environment and, for cyclohexanol dehydrogenation, the charged carbenium-ion transition state was stabilized. A higher rate was maintained with lower-acidity sodium ion–exchanged zeolites that had the same high ionic strength. Science , abh3418, this issue p. [952][1] Tailoring the molecular environment around catalytically active sites allows for the enhancement of catalytic reactivity through a hitherto unexplored pathway. In zeolites, the presence of water creates an ionic environment via the formation of hydrated hydronium ions and the negatively charged framework aluminum tetrahedra. The high density of cation-anion pairs determined by the aluminum concentration of a zeolite induces a high local ionic strength that increases the excess chemical potential of sorbed and uncharged organic reactants. Charged transition states (carbocations for example) are stabilized, which reduces the energy barrier and leads to higher reaction rates. Using the intramolecular dehydration of cyclohexanol on H-MFI zeolites in water, we quantitatively show an enhancement of the reaction rate by the presence of high ionic strength as well as show potential limitations of this strategy. [1]: /lookup/doi/10.1126/science.abh3418
领域气候变化 ; 资源环境
URL查看原文
引用统计
文献类型期刊论文
条目标识符http://119.78.100.173/C666/handle/2XK7JSWQ/328864
专题气候变化
资源环境科学
推荐引用方式
GB/T 7714
Niklas Pfriem,Peter H. Hintermeier,Sebastian Eckstein,et al. Role of the ionic environment in enhancing the activity of reacting molecules in zeolite pores[J]. Science,2021.
APA Niklas Pfriem.,Peter H. Hintermeier.,Sebastian Eckstein.,Sungmin Kim.,Qiang Liu.,...&Johannes A. Lercher.(2021).Role of the ionic environment in enhancing the activity of reacting molecules in zeolite pores.Science.
MLA Niklas Pfriem,et al."Role of the ionic environment in enhancing the activity of reacting molecules in zeolite pores".Science (2021).
条目包含的文件
条目无相关文件。
个性服务
推荐该条目
保存到收藏夹
查看访问统计
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[Niklas Pfriem]的文章
[Peter H. Hintermeier]的文章
[Sebastian Eckstein]的文章
百度学术
百度学术中相似的文章
[Niklas Pfriem]的文章
[Peter H. Hintermeier]的文章
[Sebastian Eckstein]的文章
必应学术
必应学术中相似的文章
[Niklas Pfriem]的文章
[Peter H. Hintermeier]的文章
[Sebastian Eckstein]的文章
相关权益政策
暂无数据
收藏/分享
所有评论 (0)
暂无评论
 

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。